光电子光电重合光谱提供燃料合成和转化的机理洞察,Energy & Fuels

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光电子光电重合光谱提供燃料合成和转化的机理洞察
Energy & Fuels ( IF 5.2 ) Pub Date : 2021-08-13 , DOI: 10.1021/acs.energyfuels.1c01712
Patrick Hemberger ₁ , Andras Bodi ₁ , Thomas Bierkandt ₂ , Markus Köhler ₂ , Dennis Kaczmarek ₃ , Tina Kasper ₃

Affiliation

清洁燃烧，即减少氮氧化物和烟尘排放，以及部分通过生物燃料合成实现的碳中和，是向可持续未来过渡的重要里程碑。为了克服经验性和耗时的过程优化步骤，我们需要对这些过程有详细的反应机理和化学见解。无论是在燃烧中还是在催化中，高反应性中间体，如自由基、卡宾和烯酮都会驱动化学反应。了解这些物种的命运有助于制定优化化学能转化过程的策略。这就需要先进的质谱工具来检测瞬态物质。在这次审查中，我们报告了最先进的光电子光离子符合 (PEPICO) 光谱与真空紫外 (VUV) 同步加速器辐射作为催化和燃烧研究中的高级诊断工具的应用。我们讨论了生物质转化为可持续燃料的反应机制，我们报告了使用 VUV 光电离质谱 (PIMS) 探测的木材样品的热解，并通过 PEPICO 检测对木质素模型化合物的（非）催化热解获得了深入的机械见解。PEPICO 还被证明通过揭示催化烷烃价值机制有助于对催化的机理理解。由于光电子能谱和速度图成像的应用，我们讨论了 PEPICO 检测如何推进燃烧诊断。我们报告点火的机械方面，例如燃料自由基的形成和过氧物质的氧化，并讨论污染物形成的反应途径。此外，我们放大了燃烧的基本反应并讨论了自由基氧化的异构体选择性动力学实验。还详细介绍了新发现的多环芳烃 (PAH) 形成的反应途径。最后，我们描述了当前改进 PEPICO 检测的仪器发展，并报告了与该技术相结合的创新源、反应器和反应采样方法。还详细介绍了新发现的多环芳烃 (PAH) 形成的反应途径。最后，我们描述了当前改进 PEPICO 检测的仪器发展，并报告了与该技术相结合的创新源、反应器和反应采样方法。还详细介绍了新发现的多环芳烃 (PAH) 形成的反应途径。最后，我们描述了当前改进 PEPICO 检测的仪器发展，并报告了与该技术相结合的创新源、反应器和反应采样方法。

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Photoelectron Photoion Coincidence Spectroscopy Provides Mechanistic Insights in Fuel Synthesis and Conversion

Clean combustion, i.e., the reduction of NOx and soot emissions, and carbon neutrality, achieved in part by biofuel synthesis, are major milestones in the transition to a sustainable future. To overcome empiric and time-consuming process optimization steps, we need detailed reaction mechanistic and chemical insights on these processes. Be it in combustion or in catalysis, highly reactive intermediates, such as radicals, carbenes, and ketenes drive chemical reactions. Knowing the fate of these species helps develop strategies to optimize chemical energy conversion processes. This calls for advanced mass spectrometric tools, which enable the detection of transient species. In this review, we report on the application of state-of-the-art photoelectron photoion coincidence (PEPICO) spectroscopy with vacuum ultraviolet (VUV) synchrotron radiation as advanced diagnostic tools in catalysis and combustion research. We discuss reaction mechanisms in biomass conversion to sustainable fuels, where we report on the pyrolysis of wood samples probed using VUV photoionization mass spectrometry (PIMS) and obtain deep mechanistic insights in the (non)catalytic pyrolysis of lignin model compounds with PEPICO detection. PEPICO is also shown to contribute to the mechanistic understanding of catalysis by unveiling catalytic alkane valorization mechanisms. We discuss how PEPICO detection advances combustion diagnostics, thanks to the application of photoelectron spectroscopy and velocity map imaging. We report on mechanistic aspects of ignition, such as fuel radical formation and oxidation to peroxy species, and discuss reaction pathways of pollutant formation. In addition, we zoom into the elementary reactions of combustion and discuss isomer-selective kinetics experiments on radical oxidation. Newly revealed reaction pathways to polycyclic aromatic hydrocarbon (PAH) formation are also detailed. Finally, we describe current instrumental developments to improve PEPICO detection and report on innovative sources, reactors, and reaction sampling approaches to be combined with this technique.

更新日期：2021-10-22

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